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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 433 records · Page 24
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Spin/valley pumping of resident electrons in WSe2 and WS2 monolayers

Abstract Monolayers of transition metal dichalcogenides are ideal materials to control both spin and valley degrees of freedom either electrically or optically. Nevertheless, optical excitation mostly generates excitons species with inherently short lifetime and spin/valley relaxation time. Here we demonstrate a very efficient spin/valley optical pumping of resident electrons in n-doped WSe 2 and WS 2 monolayers. We observe that, using a continuous wave laser and appropriate doping and excitation densities, negative trion doublet lines exhibit circular polarization of opposite sign and the photoluminescence intensity of the triplet trion is more than four times larger with circular excitation than with linear excitation. We interpret our results as a consequence of a large dynamic polarization of resident electrons using circular light.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Metallofullerene photoswitches driven by photoinduced fullerene-to-metal electron transfer

We report on the discovery and detailed exploration of the unconventional photo-switching mechanism in metallofullerenes, in which the energy of the photon absorbed by the carbon cage π-system is transformed to mechanical motion of the endohedral cluster accompanied by accumulation of spin density on the metal atoms. Comprehensive photophysical and electron paramagnetic resonance (EPR) studies augmented by theoretical modelling are performed to address the phenomenon of the light-induced photo-switching and triplet state spin dynamics in a series of Y x Sc 3-x N@C 80 (x = 0–3) nitride clusterfullerenes. Variable temperature and time-resolved photoluminescence studies revealed a strong dependence of their photophysical properties on the number of Sc atoms in the cluster. All molecules in the series exhibit temperature-dependent luminescence assigned to the near-infrared thermally-activated delayed fluorescence (TADF) and phosphorescence. The emission wavelengths and Stokes shift increase systematically with the number of Sc atoms in the endohedral cluster, whereas the triplet state lifetime and S 1 –T 1 gap decrease in this row. For Sc 3 N@C 80 , we also applied photoelectron spectroscopy to obtain the triplet state energy as well as the electron affinity. Spin distribution and dynamics in the triplet states are then studied by light-induced pulsed EPR and ENDOR spectroscopies. The spin–lattice relaxation times and triplet state lifetimes are determined from the temporal evolution of the electron spin echo after the laser pulse. Well resolved ENDOR spectra of triplets with a rich structure caused by the hyperfine and quadrupolar interactions with 14 N, 45 Sc, and 89 Y nuclear spins are obtained. The systematic increase of the metal contribution to the triplet spin density from Y 3 N to Sc 3 N found in the ENDOR study points to a substantial fullerene-to-metal charge transfer in the excited state. These experimental results are rationalized with the help of ground-state and time-dependent DFT calculations, which revealed a substantial variation of the endohedral cluster position in the photoexcited states driven by the predisposition of Sc atoms to maximize their spin population.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Vibronic Excitons and Conical Intersections in Semiconductor Quantum Dots

Surface defects and organic surface-capping ligands affect the photoluminescence properties of semiconductor quantum dots (QDs) by altering the rates of competing nonradiative relaxation processes. In this study, broadband two-dimensional electronic spectroscopy reveals that absorption of light by QDs prepares vibronic excitons, excited states derived from quantum coherent mixing of the core electronic and ligand vibrational states. Rapidly damped coherent wavepacket motions of the ligands are observed during hot-carrier cooling, with vibronic coherence transferred to the photoluminescent state. Furthermore, these findings suggest a many-electron, molecular theory for the electronic structure of QDs, which is supported by calculations of the structures of conical intersections between the exciton potential surfaces of a small ammonia-passivated model CdSe nanoparticle.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Elucidation of Bottom-up Growth of CaCO3 Involving Prenucleation Clusters from Structure Predictions and Decomposition of Globally Optimized (CaCO3)n Nanoclusters

Low-energy minima structures for (CaCO3)n, n = 28, are predicted using bottom-up genetic algorithms in conjunction with density functional theory electronic structure calculations, in comparison with the frozen and relaxed top-down clusters generated by cuts from the calcite, vaterite, and aragonite crystal structures. Similarities in structural motifs for the bottom-up and relaxed top-down are revealed using a fragment recognition technique. Fragment energy decomposition analysis shows that the bottom-up and relaxed top-down clusters belong to two classes of amorphous clusters with distinct intracluster energy distributions, despite their structural similarity. The bottom-up clusters with >20 formula units are surface stabilized with negative surface energy densities. In contrast, the top-down clusters are interior stabilized with positive surface energy densities. We prove that the sign of the surface energy density determines whether the nucleation reaction energy as a function of nuclear size has a maximum or a minimum. The surface-stabilized bottom-up clusters are proposed to be a type of prenucleation cluster at the minimum of the nucleation reaction energy. A mechanism for mineralization of CaCO3 involving prenucleation clusters and nonclassical growth pathway is proposed on the basis of our theoretical findings, which is consistent with previous titration experiments.

calcium carbonate, prenucleation cluster, biominer↗
DOE OSTI2026

Probing boron vacancy defects in hBN via single spin relaxometry

Spin defects in solids offer promising platforms for quantum sensing and memory due to their long coherence times and optical addressability. Here, we integrate a single nitrogen-vacancy (NV) center in diamond with scanning probe microscopy to detect, read out, and spatially map spin-based quantum sensors at the nanoscale. Using the boron vacancy ($V$$^{–}_{B}$) center in hexagonal boron nitride—an emerging two-dimensional spin system—as a model, we detect its electron spin resonance indirectly via changes in the spin relaxation time (T 1 ) of a nearby NV center, eliminating the need for optical excitation or fluorescence detection of the $V$$^{–}_{B}$. Cross-relaxation between NV and $V$$^{–}_{B}$ ensembles significantly reduces NV T1, enabling quantitative nanoscale mapping of defect densities beyond the optical diffraction limit and clear resolution of hyperfine splitting in isotopically enriched h 10 B 15 N. Our method demonstrates interactions between spin sensors in 3D and 2D materials, establishing NV centers as versatile probes for characterizing otherwise inaccessible spin defects.

Quantum metrology↗
DOE OSTI2022

A MeerKAT-meets-LOFAR study of MS 1455.0 + 2232: a 590 kiloparsec ‘mini’-halo in a sloshing cool-core cluster

ABSTRACT Radio mini-haloes are poorly understood, moderately extended diffuse radio sources that trace the presence of magnetic fields and relativistic electrons on scales of hundreds of kiloparsecs, predominantly in relaxed clusters. With relatively few confirmed detections to-date, many questions remain unanswered. This paper presents new radio observations of the galaxy cluster MS 1455.0+2232 performed with MeerKAT (covering the frequency range 872−1712 MHz) and LOFAR (covering 120−168 MHz), the first results from a homogeneously selected mini-halo census. We find that this mini-halo extends for ∼590 kpc at 1283 MHz, significantly larger than previously believed, and has a flatter spectral index (α = −0.97 ± 0.05) than typically expected. Our X-ray analysis clearly reveals a large-scale (254 kpc) sloshing spiral in the intracluster medium. We perform a point-to-point analysis, finding a tight single correlation between radio and X-ray surface brightness with a super-linear slope of $b_{\rm 1283\, MHz} = 1.16^{+0.06}_{-0.07}$ and $b_{\rm 145\, MHz} = 1.15^{+0.09}_{-0.08}$; this indicates a strong link between the thermal and non-thermal components of the intracluster medium. Conversely, in the spectral index/X-ray surface brightness plane, we find that regions inside and outside the sloshing spiral follow different correlations. We find compelling evidence for multiple sub-components in this mini-halo for the first time. While both the turbulent (re-)acceleration and hadronic scenarios are able to explain some observed properties of the mini-halo in MS 1455.0+2232, neither scenario is able to account for all the evidence presented by our analysis.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Time-resolved resonant inelastic x-ray scattering in a pumped Mott insulator

Collective excitations contain rich information about photoinduced transient states in correlated systems. In a Mott insulator, charge degrees of freedom are frozen, but can be activated by photodoping. The energy-momentum distribution of the charge excitation spectrum reflects the propagation of charge degrees of freedom and provides information about the interplay among various intertwined instabilities on the timescale set by the pump. To reveal charge excitations out of equilibrium, here we simulate time-resolved x-ray absorption and resonant inelastic x-ray scattering using a Hubbard model. After pumping, the former resolves photodoping, while the latter characterizes the formation, dispersion, weight, and nonlinear effects of collective excitations. Intermediate-state information from time-resolved resonant inelastic x-ray scattering (trRIXS) can be used to decipher the origin of these excitations, including bimagnons, Mott-gap excitations, doublon and single-electron in-gap states, and anti-Stokes relaxation during an ultrafast pump. This paper provides a theoretical foundation for existing and future trRIXS experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Ultrafast optical modulation of vibrational strong coupling in ReCl(CO) 3 (2,2-bipyridine)

Polaritons – hybrid light-matter states formed from the strong coupling of a bright molecular transition with a confined photonic mode – may offer new opportunities for optical control of molecular behavior. Vibrational strong coupling (VSC) has been reported to impact ground-state chemical reactivity, but its influence on electronic excited-state dynamics remains unexplored. Here, we take a first step towards excited-state VSC by demonstrating optical modulation of the ReCl(CO) 3 (bpy), (bpy = 2,2-bipyridine) complex under VSC using femtosecond ultraviolet (UV)-pump/infrared (IR)-probe spectroscopy. We establish ground-state VSC of ReCl(CO) 3 (bpy) in a microfluidic Fabry-Pérot cavity equipped with indium tin oxide (ITO)-coated mirrors. ITO is effectively dichroic as it is reflective in the IR and transmissive in the UV-visible and therefore minimizes optical interference. Excitation with UV pump light drives ReCl(CO) 3 (bpy) into a manifold of electronic excited states that subsequently undergo non-radiative relaxation dynamics. We probe the transient response of the strongly-coupled system in the mid-IR, observing both Rabi contraction and cavity-filtered excited-state absorption signatures. We reconstruct the intrinsic response of intracavity molecules from the transient cavity transmission spectra to enable quantitative comparison with extracavity control experiments. We report no changes in the excited-state dynamics of ReCl(CO) 3 (bpy) under ground-state VSC. However, we do observe significant amplification of transient vibrational signals due to classical cavity-enhanced optical effects. This effort lays the groundwork to pursue direct excited-state VSC aimed at modulating photochemical reactivity.

cavity-enhanced spectroscopy↗
NASA NTRS1980

Some features of inverted-V events as seen from simulated double layers

Results from a numerical simulation of a double layer show some features similar to those of inverted-V events. The strong heating of thermal and precipitating electrons is observed along with extremely low frequency fluctuations found during inverted-V events. It is suggested that after the acceleration of auroral electrons by the double layer, the precipitating free electrons are heated by the nonlinear effects of the electron beam plasma instability. Fluctuations and pulsations of auroral electron fluxes during auroral events are caused by a relaxation type of oscillation. The finite extent of one dimensional plasma is simulated by solving the Vlasov and Poisson equations as an initial and boundary value problem.

Singh, N.↗
NASA NTRS1986

Crack Growth in Single-Crystal Silicon

Report describes experiments on crack growth in single-crystal silicon at room temperature in air. Crack growth in (111) cleavage plane of wafers, 50 by 100 by 0.76 mm in dimension, cut from Czochralski singlecrystal silicon studied by double-torsion load-relaxation method and by acoustic-emission measurements. Scanning electron microscopy and X-ray topography also employed. Results aid in design and fabrication of silicon photovoltaic and microelectronic devices.

Chen, C. P.↗
NASA NTRS1990

Pulsed-discharge carbon dioxide lasers

The purpose is to attempt a general introduction to pulsed carbon dioxide lasers of the kind used or proposed for laser radar applications. Laser physics is an excellent example of a cross-disciplinary topic, and the molecular spectroscopy, energy transfer, and plasma kinetics of the devices are explored. The concept of stimulated emission and population inversions is introduced, leading on to the molecular spectroscopy of the CO2 molecule. This is followed by a consideration of electron-impact pumping, and the pertinent energy transfer and relaxation processes which go on. Since the devices are plasma pumped, it is necessary to introduce a complex subject, but this is restricted to appropriate physics of glow discharges. Examples of representative devices are shown. The implications of the foregoing to plasma chemistry and gas life are discussed.

Willetts, David V.↗
NASA NTRS1994

Pulsed acceleration in solar flares

We study the nonlinear dynamics of particle acceleration in solar flares by analyzing the time series of various quasi-periodic radio signatures during flares. In particular we present the radio and hard X-ray data of three flares which suppport the following tentative conclusions: (1) Particle acceleration and injection into magnetic structures occurs intrinsically in a pulsed mode (with a typical period of 1-2 s), produced by a single, spatially coherent, nonlinear system, rather than by a stochastic system with many spatially independent components ('statistical flare' produced by a fragmented primary energy release). (2) The nonlinear (quasi-periodic) mode of pulsed particle acceleration and injection into a coronal loop can be stabilized by phase locking with an MHD wave (oscillation) mode, if both periods are close to each other. (3) Pulsed injection of electron beams into a coronal loop may trigger nonlinear relaxational oscillations of wave-particle interactions. This is particularly likely when the limit cycles of both systems are similar.

Aschwanden, Markus J.↗
NASA NTRS2019

Plasma Science in Planetary Entry

Spacecraft entering a planetary atmosphere dissipate a great deal of energy into the surrounding gas. In the frame of reference of the vehicle, the atmospheric gas suddenly decelerates from hypersonic (Mach ~5-50) to subsonic velocities. The kinetic energy of the gas is rapidly converted to thermal and chemical energy, forming a bow shock behind which a plasma with energies on the order of one electron volt (eV) is produced. The resulting shock layer relaxes from strong thermal non-equilibrium that is translationally hot but internally cold and un-ionized toward a thermochemically equilibrated plasma over a distance of a few centimeters. Composition is dependent upon the planetary atmosphere – Air for Earth, CO2/N2 for Mars and Venus, N2/CH4 for Titan and H2/He/CH4 for Saturn, Neptune and Jupiter. Typical velocities of entry may range from 3-7 km/s (4-25 MJ/kg) for Titan/Mars, 8-14 km/s (30-100 MJ/kg) for Earth/Venus, and 25-40 km/s (300-800 MJ/kg) for outer planets. The equilibrium plasmas produced from these conditions are highly dissociated (up to and above 99%) and ionized (0.1- 15%), with temperatures from 7,000-15,000K and pressures from 0.1-1.0 bar. Understanding the behavior of these plasmas – the way in which they approach equilibrium, how they radiate, and how they interact with materials – is an active area of research necessitated by requirements to predict and test the performance of thermal protection systems (TPS) that enable spacecraft to deliver scientific instruments, and people, to foreign worlds and back to Earth. The endeavor is a multi-physics problem, with key processes highlighted in Fig. 1. This white paper describes the current state of the art in simulating shock layer plasmas both computationally and in ground test facilities. Gaps requiring further research and development are identified.

Cruden, Brett A.↗
DOE OSTI2023

Substrate effects on spin relaxation in two-dimensional Dirac materials with strong spin-orbit coupling

Understanding substrate effects on spin dynamics and relaxation is of key importance for spin-based information technologies. However, the key factors that determine such effects, in particular for materials with strong spin-orbit coupling (SOC), have not been well understood. Here we performed first-principles real-time density-matrix dynamics simulations with SOC and the electron phonon and electron-impurity scattering for spin lifetimes (τ s ) of supported/free-standing germanene, a prototypical strong SOC 2D Dirac material. We show that the effects of different substrates on τ s can surprisingly differ by two orders of magnitude. We find that substrate effects on τ s are closely related to substrate-induced modifications of the SOC-field anisotropy, which changes the spin flip scattering matrix elements. We propose a new electronic quantity, named spin-flip angle θ ↑↓ , to characterize spin relaxation through intervalley spin-flip scattering. We find that $τ^{-1}_s$ is approximately proportional to the averaged value of sin 2 (θ ↑↓ /2), which serves as a guiding parameter of controlling spin relaxation.

36 MATERIALS SCIENCE↗
DOE OSTI2020

The Role of Surface Oxygen Vacancies in BiVO 4

Bismuth vanadate (BiVO 4 ) is a widely studied oxide in solar water splitting, known for its ease of synthesis, high charge extraction yields, and advantageous band alignment with water. We present a combined first-principles and experimental study of the electronic structure of the (010) surface of BiVO 4 aimed at disentangling the impact of the surface and bulk oxygen vacancies on the electronic structure and transport properties. We found that oxygen vacancies are deep donors at the surface as they are in the bulk; our calculations on defect and polaron formation energies suggest that, while polarons formed from oxygen vacancies in the bulk can contribute to conductivity, those at the surface likely do not. Our results also show that out-of-plane structural relaxations at the surface contribute to the relatively immobile nature of electron polarons derived from surface oxygen vacancies. The structural model derived from first-principles calculation was validated by comparing computed results with experimental measurements of single-crystal and epitaxially grown single-crystalline BiVO 4 samples. Finally, we also found a reasonably good agreement between our calculated and measured work functions for BiVO 4 samples with and without oxygen vacancies.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Lattice vacancy migration barriers in Fe-Ni alloys, and an indication as to why Ni atoms diffuse slowly: A first-principles study

Lattice vacancy migration barriers in ferromagnetic Fe 𝑥 ⁢Ni 1−𝑥 alloys (0.4 ≤ 𝑥 ≤ 0.6) are accurately quantified within the framework of ab initio electronic structure calculations using the nudged elastic band (NEB) method. Both the atomically disordered (A1) fcc phase, as well as the atomically ordered, tetragonal L⁢1 0 phase—which is under consideration as a material for a rare-earth-free gap magnet for advanced engineering applications—are investigated. Across an ensemble of NEB calculations performed on supercell configurations spanning a range of compositions and containing disordered, partially ordered, and fully ordered structures, we find that Ni-vacancy interchanges encounter significantly higher energetic barriers than do Fe-vacancy interchanges. We contend that this aspect is a key factor in determining the differences in mobility between Fe and Ni atoms in this ferromagnetic alloy. Moreover, we are able to interpret these findings in terms of the ferromagnetic alloy's underlying spin-polarized electronic structure. Specifically, we report a coupling between the size of local lattice distortions and the magnitude of the local electronic spin polarization around vacancies. This causes Fe atoms to relax into lattice vacancies, while Ni atoms remain rigidly fixed to their original lattice positions. These results give atomic-scale insight into the longstanding experimental observation that Ni exhibits remarkably slow atomic diffusion in Fe-Ni alloys.

density functional theory↗